Abstract:The energy disorder that arises from colloidal quantum dot (CQD) polydispersity limits the open-circuit voltage (V ) and efficiency of CQD photovoltaics. This energy broadening is significantly deteriorated today during CQD ligand exchange and film assembly. Here, a new solution-phase ligand exchange that, via judicious incorporation of reactivity-engineered additives, provides improved monodispersity in final CQD films is reported. It has been found that increasing the concentration of the less reactive speci… Show more
“…Monodisperse colloidal NCs as a light-absorbing layer provide reduced energetic disorder and band tail broadening, both of which are urgently required to improve solar cell performance. [24][25][26][27][28] The use of oleylamine in previous oleate-based synthetic routes enables improved monodispersity of AgBiS 2 NCs because the oleylamine not only helps the Ag precursor to completely dissolve, but also provides an efficient surface passivation of the AgBiS 2 NCs with oleic acid. 28 Surface ligands with various functional groups such as thiol, amine, and carboxylate greatly affect the chemical and physical properties of the resultant semiconducting colloidal NCs.…”
Ternary silver bismuth sulfide (AgBiS 2) colloidal nanocrystals (NCs) have been recognized as a photovoltaic absorber for environmentally-friendly and lowtemperature-processed thin film solar cells. However, previous synthetic methods involving hot injection of sulfur precursors into metal oleate precursor solutions do not provide a balance between nucleation and growth, leading to AgBiS 2 NCs with broad size distributions. Here, we demonstrate the modified synthetic route that size distribution of AgBiS 2 NCs can be improved by pre-adding the non-coordinating 1-octadecene (ODE) solvent into metal precursor solutions, leading to controlled concentration of coordinating oleic acid with improved hot-injection synthetic conditions. The addition of ODE as a non-coordinating solvent to metal precursor/oleic acid solution significantly suppresses variations in the concentration of coordinating oleic acid after injection of the sulfur precursor solution, leading to a homogenous reaction between the metal and sulfur precursors. For photovoltaic devices fabricated using the resultant AgBiS 2 NCs, the champion device shows power conversion efficiency (PCE) of 5.94% with an open-circuit voltage (V OC) of 0.52 V. This performance is better than that a control device (PCE of 5.50% and V OC of 0.49 V) because of the reduced energetic disorder and band tail broadening originating from the uniformly-sized AgBiS 2 NCs.
“…Monodisperse colloidal NCs as a light-absorbing layer provide reduced energetic disorder and band tail broadening, both of which are urgently required to improve solar cell performance. [24][25][26][27][28] The use of oleylamine in previous oleate-based synthetic routes enables improved monodispersity of AgBiS 2 NCs because the oleylamine not only helps the Ag precursor to completely dissolve, but also provides an efficient surface passivation of the AgBiS 2 NCs with oleic acid. 28 Surface ligands with various functional groups such as thiol, amine, and carboxylate greatly affect the chemical and physical properties of the resultant semiconducting colloidal NCs.…”
Ternary silver bismuth sulfide (AgBiS 2) colloidal nanocrystals (NCs) have been recognized as a photovoltaic absorber for environmentally-friendly and lowtemperature-processed thin film solar cells. However, previous synthetic methods involving hot injection of sulfur precursors into metal oleate precursor solutions do not provide a balance between nucleation and growth, leading to AgBiS 2 NCs with broad size distributions. Here, we demonstrate the modified synthetic route that size distribution of AgBiS 2 NCs can be improved by pre-adding the non-coordinating 1-octadecene (ODE) solvent into metal precursor solutions, leading to controlled concentration of coordinating oleic acid with improved hot-injection synthetic conditions. The addition of ODE as a non-coordinating solvent to metal precursor/oleic acid solution significantly suppresses variations in the concentration of coordinating oleic acid after injection of the sulfur precursor solution, leading to a homogenous reaction between the metal and sulfur precursors. For photovoltaic devices fabricated using the resultant AgBiS 2 NCs, the champion device shows power conversion efficiency (PCE) of 5.94% with an open-circuit voltage (V OC) of 0.52 V. This performance is better than that a control device (PCE of 5.50% and V OC of 0.49 V) because of the reduced energetic disorder and band tail broadening originating from the uniformly-sized AgBiS 2 NCs.
“…The replacement of the long-chain ligands by the short-chain conductive ligands can lead to a stripped CQD surface, resulting in CQD fusion [29,49]. The polydispersity of PbS CQDs can be reduced by controlling the reactivity of ligands during the ligand exchange process [50]. For this purpose, ammonium acetate (AA, reactive species) and tetrabutylammonium acetate (TBAA, less reactive species) mixtures were employed for the solution-phase ligand exchange, and these simultaneously provided improved surface passivation and charge transport with preserved the homogeneity of the PbS CQDs.…”
Colloidal quantum dots (CQDs) are considered as next-generation semiconductors owing to their tunable optical and electrical properties depending on their particle size and shape. The characteristics of CQDs are mainly governed by their surface chemistry, and the ligand exchange process plays a crucial role in determining their surface states. Worldwide studies toward the realization of high-quality quantum dots have led to advances in ligand exchange methods, and these procedures are usually carried out in either solid-state or solution-phase. In this article, we review recent advances in solid-state and solution-phase ligand exchange processes that enhance the performance and stability of lead sulfide (PbS) CQD solar cells, including infrared (IR) CQD photovoltaics.
“…Ein derartiger Ligandenaustausch ergab eine bessere Passivierung mit höherem Halogenidgehalt und ermöglichte die Herstellung von Bauelementen mit dickerer aktiver Schicht, die einen größeren Anteil des einfallenden Sonnenlichts absorbieren kann. Außerdem gab es verschiedene Versuche, die Grenzfläche zwischen dem halbleitenden Elektronentransportmaterial (d. h. ZnO und TiO 2 ) und kolloidalen QD‐Tinten unter Verwendung selbstorganisierender Monolagen von organischen Molekülen zu verbessern, 1) um eine bessere Bandanpassung unter Verwendung gemischter QD‐Tinten über kolloidalen Ligandenaustausch zu ermöglichen; 2) um die Leerlaufspannung zu erhöhen, indem die aus der Polydispersität der kolloidalen QDs resultierende Energiestörung über lösungsbasierten Ligandenaustausch durch Einbau von Additiven mit manipulierter Reaktivität verringert wird; und 3) um ZnO‐Elektroden für eine bessere Ladungsinjektion unter Verwendung von Halogeniden zu passivieren . In der Folge haben PV‐Bauelemente mit verarmtem Heteroübergang auf Bleichalkogenidbasis dauerhaft einen Wirkungsgrad von über 10 % gezeigt.…”
Section: Solarzellen Auf Bleichalkogenid‐basisunclassified
Quantenpunkte (QDs) von Bleichalkogeniden (z. B. PbS, PbSe und PbTe) sind nahinfrarotaktive Materialien, die großes Potenzial für einen breiten Bereich von Anwendungen wie Photovoltaik, Optoelektronik, Sensorik und Bioelektronik zeigen. Oberflächenliganden spielen eine wesentliche Rolle bei der Herstellung und postsynthetischen Modifizierung von QDs sowie bei deren Einsatz in Anwendungen. Daher ist ein gutes Verständnis des Einflusses von Oberflächenliganden auf die Synthese und Eigenschaften von QDs für deren Anwendungen in verschiedenen Bauelementen unerlässlich. Der vorliegende Aufsatz beschäftigt sich mit der Anwendung kolloidaler Synthesetechniken zur Herstellung von bleichalkogenidbasierten QDs. Der Schwerpunkt liegt auf dem Einfluss von Oberflächenliganden auf die QD‐Synthese sowie dem Ligandenaustausch in Lösung. Angesichts der Bedeutung von Bleichalkogenid‐QDs als möglichen Lichtsammlern richten wir unsere Aufmerksamkeit besonders auf die aktuellen Fortschritte von PV‐Anwendungen mit diesen QDs.
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